Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and e...Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and exchangecorrelation effects but also the interference between the dynamics of different electron wave packets.展开更多
The tensile strain in inorganic perovskite films induced by thermal annealing is one of the primary factors contributing to the inefficiency and instability of inorganic perovskite solar cells(IPSCs),which reduces the...The tensile strain in inorganic perovskite films induced by thermal annealing is one of the primary factors contributing to the inefficiency and instability of inorganic perovskite solar cells(IPSCs),which reduces the defect formation energy.Here,a flexible molecule 5-maleimidovaleric acid(5-MVA)was introduced as a strain buffer to release the residual strain of CsPbI_(2.85)Br_(0.15)perovskite.Maleic anhydride and carboxyl groups in 5-MVA interact strongly with the uncoordinated Pb^(2+)through Lewis acid-base reaction,thus tightly“pull”the perovskite lattice.The in-between soft carbon chain increased the structural flexibility of CsPbI_(2.85)Br_(0.15)perovskite materials,which effectively relieved the intrinsic internal strain of CsPbI_(2.85)Br_(0.15),resisted the corrosion of external strain,and also reduced the formation of defects such as VIand Pb0.In addition,the introduction of 5-MVA improved crystal quality,passivated residual defects,and narrowed energy level barriers.Eventually,power conversion efficiency(PCE)of NiOxbased inverted IPSCs increased from 19.25%to 20.82%with the open-circuit voltage enhanced from 1.164 V to 1.230 V.The release of strain also improved the stability of CsPbI_(2.85)Br_(0.15)perovskite films and devices.展开更多
An in-depth understanding of the hydration mechanism of tricalcium silicate is an important basis for optimizing cement strength development.In this study,the adsorption of water molecules onto the M3-C3S(001)surface ...An in-depth understanding of the hydration mechanism of tricalcium silicate is an important basis for optimizing cement strength development.In this study,the adsorption of water molecules onto the M3-C3S(001)surface at different water coverage levels(θ=1/5,2/5,3/5,4/5,and 1)was investigated using first-principles calculations.The results demonstrate that the conclusions obtained for single water molecule adsorption cannot be fully applied to multiple water molecule adsorption.The total adsorption energies become more negative with increasing water coverage,while the average adsorption energy of each water molecule becomes more positive with increasing water coverage.The water–water interactions reduce the water–surface interactions and are responsible for the anticooperative adsorption of multiple water molecules onto M3-C_(3)S(001).The formation of Ca–OH(–Ca)bonds favors the detachment of Ca from co-valent oxygen,which reveals the significant role of dissociative adsorption.This work aims to extend the water adsorption study on M3-C3S(001)from single water molecule adsorption to multiple water molecule adsorption,providing more detailed insights into the initial water reaction on the C3S surface.展开更多
The ring has been a romantic fascination throughout the ages,embodying not only beauty and order but also harboring numerous undisclosed properties awaiting discovery.In the realm of supramolecular chemistry,macrocycl...The ring has been a romantic fascination throughout the ages,embodying not only beauty and order but also harboring numerous undisclosed properties awaiting discovery.In the realm of supramolecular chemistry,macrocycles,with a cyclic structure and a central cavity like a doughnut,captivate the attention of scientists[1].In 1967,Pedersen's groundbreaking revelation that alkali metal ions could"fall into"the cavities of a cyclic ether named crown ether,even in organic solvents,unveiled a novel universe of macrocycle chemistry.Since then,numerous macrocyclic structures in nature have been discovered,isolated,and scrutinized.Drawing inspiration from nature,chemists endeavor to explore the vast potential of macrocyclic compounds by designing and synthesizing artificial macrocycles with diverse structural features and recognition properties.展开更多
In recent years,the ternary strategy of adding a vip molecule to the active layer has been proven to be effective for improving the performance of organic solar cells(OSCs).Isomerization engineering of the vip mol...In recent years,the ternary strategy of adding a vip molecule to the active layer has been proven to be effective for improving the performance of organic solar cells(OSCs).Isomerization engineering of the vip molecule is a simple method to increase the amount of promising material,but there are only limited reports,and the structure-property relationships are still unclear.In this work,we synthesized three isomers named BTA5-F-o,BTA5-F-m,and BTA5-F-p,with different fluorine substitution positions,to study the influence of isomerization on the photovoltaic performance.After introducing them as the third components to the classic host system PM6:Y6,all three ternary devices showed improved power conversion efficiency(PCEs)compared to the binary system(PCE of 17.46%).The ternary OSCs based on BTA5-F-o achieved a champion PCE of 19.11%,while BTA5-F-m and BTA5-F-p realized PCEs of 18.65%and 18.45%,respectively.Mechanism studies have shown that the dipole moment of the BTA5-F-o end group is closer to that of the Y6 end group,despite the three isomers with almost identical energy levels and optical properties.It is indicated that the electron attraction ability of BTA5-F-o best matches that of Y6,which leads to the higher charge mobility,less charge recombination,and stronger exciton dissociation and extraction ability in the ternary blend system.This study suggests that rationally adjusting the position of substituents in the terminal group can be an effective way to construct nonfullerene vip acceptors to achieve highly efficient ternary OSCs.展开更多
Enhanced mass concentrations of aromatic-derived secondary organic aerosol(SOA)are frequently observed during humid-haze events.However,the influencing mechanism of relative humidity(RH)in aromatic-derived SOA formati...Enhanced mass concentrations of aromatic-derived secondary organic aerosol(SOA)are frequently observed during humid-haze events.However,the influencing mechanism of relative humidity(RH)in aromatic-derived SOA formation remains incompletely understood.Here,the RH dependence of SOA formation in the presence of NOx was explored by a series of chamber experiments for toluene(TOL)and 1,3,5-trimethylbenzene(TMB)photooxidation.The yield of TOL SOA and TMB SOA increased by 221%and 52%with increasing RH from~8%to~70%,respectively.Analytical results from a high-resolution mass spectrometer showed that SOA constituents with high oxygen content(O/C>0.6)were more abundant in SOA formed in the~70%RH experiment.The elevated yields and O/C of SOA could be attributed to the promoted formation and particle-phase diffusivity of highly oxidized molecules.In addition,in comparison with TMB,TOL could produce more unsaturated aldehydes,which are oxidized into carboxylic acids with high O/C,leading to a more sensitive response of TOL SOA formation to the change in RH.Our work provides mechanistic insights into RH roles in aromatic SOA formation and is helpful for a better understanding of humid-haze events.展开更多
This paper provides a systematic review of Matrix-Assisted Laser Desorption/Ionization-Mass Spectrometry Imaging(MALDI-MSI),encompassing its technical principles,experimental workflows,matrix optimization strategies,a...This paper provides a systematic review of Matrix-Assisted Laser Desorption/Ionization-Mass Spectrometry Imaging(MALDI-MSI),encompassing its technical principles,experimental workflows,matrix optimization strategies,and recent advancements in plant science applications.It highlights the method's groundbreaking applications in spatial mapping of plant metabolites,dynamic hormone monitoring,and functional studies of tissue microdomains,while offering critical insights into current technical limitations and future research directions.展开更多
Acceptor-donor-acceptor(A-D-A)type molecules,of which the novel non-fused azacyclic end-group pyrazoli-nones were modified with chlorine substitution on the phenyl ring,were synthesized.The non-fused azacyclic end-gro...Acceptor-donor-acceptor(A-D-A)type molecules,of which the novel non-fused azacyclic end-group pyrazoli-nones were modified with chlorine substitution on the phenyl ring,were synthesized.The non-fused azacyclic end-group py-razolinones have the advantages of simple synthesis steps,low cost and environmental friendliness,compared to the classical end-group dicyanomethyleneindianone.The properties of the synthesized A-D-A type molecules with non-fused azacyclic end groups were characterized by theoretical calculation,UV-vis absorption,cyclic voltammetry,X-ray diffraction and space charge limited current.It is shown that the strong UV-vis absorptions of the synthesized A-D-A type molecules are located in the wavelength range of 500~700 nm,with a moderate band gap of nearly 1.7 eV.At the same time,the influence of end-group chlorination on the properties of A-D-A type molecules was compared and explored.It is proven that this kind of A-D-A type molecule with non-fused azacyclic end groups has the potential to be applied as interfacial modified layer of the active layer in perovskite solar cell devices.展开更多
CRISPR-based tran-scription regulators(CRISPR-TRs)have revolutionized the field of synthetic biol-ogy by enabling tar-geted activation or repression of any de-sired gene.However,the majority of exist-ing inducible CRI...CRISPR-based tran-scription regulators(CRISPR-TRs)have revolutionized the field of synthetic biol-ogy by enabling tar-geted activation or repression of any de-sired gene.However,the majority of exist-ing inducible CRISPR-TRs are limited by their dependence on specific sequences,which restricts their flex-ibility and controllability in genetic engineering applications.In this study,we proposed a novel strategy to construct sequence-independent inducible CRISPR-TRs,which is achieved by the design of stem loop 2 in the single guide RNA(sgRNA).Under this strategy,by utiliz-ing toehold-mediated strand displacement(TMSD)reactions between small endogenous molecules(miR-20a and TK1 mRNA)and bridge RNA(bRNA)to link bRNA with sgRNA,we achieved synergistic transcriptional activation of VP64 and p65-HSF1 in response to en-dogenous molecules.To enable response to exogenous molecules,we added response se-quences and bRNA sequences to the 5'end of sgRNA to block sgRNA activity,and achieved activation of sgRNA by shearing the response sequence,called sequential unlimited interlock-ing(SUI).Compared with conventional sequence-restricted interlocking(spacer-blocking hairpin(SBH)),the transcriptional activation ratio between response and non-response to the Cas6A protein using our approach was increased by 2.28-fold.Our work presents a modular and versatile framework for endogenous and exogenous molecule-responsive CRISPR-TRs in mammalian cells,without limitations imposed by sequence dependence.展开更多
Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from...Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from the cathode side.These challenges lead to poor cycle stability and severe self-discharge.From the fabrication and cost point of view,it is technologically more viable to deploy electrolyte engineering than electrode protection strategies.More importantly,a synchronous method for modulation of both cathode and anode is pivotal,which has been often neglected in prior studies.In this work,cationic poly(allylamine hydrochloride)(Pah^(+))is adopted as a low-cost dual-function electrolyte additive for ZIBs.We elaborate the synchronous effect by Pah^(+)in stabilizing Zn anode and immobilizing polyiodide anions.The fabricated Zn-iodine coin cell with Pah^(+)(ZnI_(2) loading:25 mg cm^(−2))stably cycles 1000 times at 1 C,and a single-layered 3.4 cm^(2) pouch cell(N/P ratio~1.5)with the same mass loading cycles over 300 times with insignificant capacity decay.展开更多
Exploring multifunctional interfacial modifiers is an effective approach to addressing interface issues in perovskite solar cells(PSCs)and improving device performance and stability.While most interfacial modifiers fo...Exploring multifunctional interfacial modifiers is an effective approach to addressing interface issues in perovskite solar cells(PSCs)and improving device performance and stability.While most interfacial modifiers focus on passivating defects at the interfaces,there has been limited investigation into the relationship between molecular design and interfacial charge dynamics.This work introduces resonance molecules with a push-pull effect for interfacial modification,allowing for synergistic regulation of passivation effects and charge dynamics.Specifically,FCz-PO,which includes an electron-withdrawing fluorine atom,exhibits superior passivation but poor molecular stacking and charge extraction.In contrast,MCz-PO,featuring an electron-donating methoxy group,provides effective passivation,wellordered molecular packing,and efficient charge extraction and transport.Consequently,PSCs using MCz-PO achieve high power conversion efficiency(PCE)of 24.74%and excellent operational stability.This study suggests that resonance structures can be an effective molecular design strategy for developing interfacial modifiers with both strong passivation capabilities and well-regulated charge dynamics.展开更多
Spiral patterns widely exist in both macroscopic and microscopic systems such as hearts,bacteria,and active matters but have never been reported at molecular length scale.The emergence of spiral patterns has considera...Spiral patterns widely exist in both macroscopic and microscopic systems such as hearts,bacteria,and active matters but have never been reported at molecular length scale.The emergence of spiral patterns has considerable impacts on the trajectories of the objects and thus usually relates to various physical,chemical,biological and physiological processes.In this paper,we show that,down to the length scale of only several Angstroms,asymmetric molecules exhibit spiral patterns in their trajectories within finite time based on the under-damped Langevin equation and demonstrated by molecular dynamics simulation.The key to this observation lies in the asymmetric molecular architecture that leads to a translation-rotation coupling.This finding enriches the knowledge of spiral patterns to the molecular length scale,provides a new insight into the understanding of various processes at the molecular level,and may evoke new ideas on the understanding of the vortices in turbulence.展开更多
The presence of residual alkaline compounds in the ultrahigh-nickel layered oxide cathodes(LiNi_(x)Co_(y)Mn_(1−x−y)O_(2),x≥_(0.9))aggravates structural degradation,increases surface reactivity,and promotes slurry gel...The presence of residual alkaline compounds in the ultrahigh-nickel layered oxide cathodes(LiNi_(x)Co_(y)Mn_(1−x−y)O_(2),x≥_(0.9))aggravates structural degradation,increases surface reactivity,and promotes slurry gelation,leading to the capacity decay of batteries with these cathodes and complicating their manufacturing.Traditional approaches for addressing this issue,including direct removal,coverage,and utilization,are complex and require surface regeneration.Herein,we propose neutralizing residual alkaline compounds with 3-thiopheneboronic acid(3-TBA)to improve the performance of LiNi_(0.9)5Co_(0.04)Mn_(0.01)O_(2)(NCM)cathode material,a facile strategy that does not require any post-treatment.The suggested reaction yields a uniform and thin organic-modified layer on the surface of the NCM cathode,improving its chemical stability toward the electrolyte,as demonstrated by multiple characterization methods.The modified NCM cathode exhibited impressive cyclic and rate performances,achieving a capacity retention of 83.34%after 200 cycles at 1.0 C and a specific capacity of 162.00 mAh·g^(−1) at 10.0 C.Most importantly,the proposed approach can efficiently suppress unfavorable phase transitions,severe electrolyte degradation,and CO_(2) gas evolution,improving the application potential of ultrahigh-nickel layered oxide cathode materials.展开更多
We propose a scheme for dual-species deceleration and trapping of a cold atom–molecule mixture by a frequency chirping stimulated force.We study the stimulated force exerted on Mg F and Rb using optical Bloch equatio...We propose a scheme for dual-species deceleration and trapping of a cold atom–molecule mixture by a frequency chirping stimulated force.We study the stimulated force exerted on Mg F and Rb using optical Bloch equations based on a direct numerical solution for the time-dependent density matrix.We analyze the relationship between the frequency chirping rate and the number of Mg F molecules and Rb atoms.In addition,we study the dynamical process of molecular deceleration and the effect of transverse diffusion.Monte–Carlo simulations show that buffer-gas-cooled Mg F and Rb beams,with initial velocities of 200 m/s and 130 m/s respectively,can be decelerated to less than 10 m/s.This is achieved with laser powers of as low as 357 m W for Mg F and 10 m W for Rb per traveling wave.The rapid deceleration minimizes molecular loss due to transverse diffusion during the deceleration process.The estimated number of molecules that can be trapped in a magneto-optical trap(MOT)is about 9.0×10^(6),which is an order of magnitude larger than the number of Mg F molecules decelerated by the spontaneous radiation force.The results offer a promising starting point for further studies of sympathetic cooling.展开更多
Recent theoretical verification of self-similar and dissipative pure-quartic solitons(PQSs)emphasized the similarity between PQS lasers and conventional fiber lasers,but the unique equilibrium mechanism hinders the fo...Recent theoretical verification of self-similar and dissipative pure-quartic solitons(PQSs)emphasized the similarity between PQS lasers and conventional fiber lasers,but the unique equilibrium mechanism hinders the formation of PQS molecules in normal fourth-order dispersion(FOD)regimes.In this paper,we investigated the effect of filters on shaping PQSs in normal FOD based on a passively mode-locked fiber laser model.A bandpass filter eliminates the time pedestal of dissipative PQSs,thus realizing a multi-pulsing state.When the filter bandwidth is appropriate,the effective spectral filtering effect can lower the pulse splitting threshold and enable the coherent restoration from chaotic PQSs to PQS molecules.Additionally,changing the central wavelength of the filter can generate PQSs and PQS molecules with asymmetric intensity distributions.These results are important guides for the manipulation of PQSs and the construction of high repetition-frequency fiber lasers.展开更多
We present a theoretical approach to achieve sub-Doppler cooling of magnesium fluoride(Mg F) molecules by tuning the AC Stark shift with a blue-detuned laser. We study three blue-detuned magneto–optical trapping(MOT)...We present a theoretical approach to achieve sub-Doppler cooling of magnesium fluoride(Mg F) molecules by tuning the AC Stark shift with a blue-detuned laser. We study three blue-detuned magneto–optical trapping(MOT) schemes by using the Bayesian optimization method with the optical Bloch equations. We perform a comprehensive analysis of the relationship between the force in the MOT and the velocities and positions of the Mg F molecules. Monte–Carlo simulations show that our MOT schemes can achieve a temperature as low as 28 μK and a density as high as 4.0 × 10^(8)cm^(-3) at the conditions of a ratio of two laser intensities of 2:7, a detuning of 3Γ and a polarization configuration of σ^(-)-σ^(+). These results provide a clear way for transferring a large number of Mg F molecules into a conservative trap to enhance the subsequent cooling such as evaporative or sympathetic cooling.展开更多
The architectural design of redox-active organic molecules and the modulation of their electronic properties significantly influence their application in energy storage systems within aqueous environments.However,thes...The architectural design of redox-active organic molecules and the modulation of their electronic properties significantly influence their application in energy storage systems within aqueous environments.However,these organic molecules often exhibit sluggish reaction kinetics and unsatisfactory utilization of active sites,presenting significant challenges for their practical deployment as electrode materials in aqueous batteries.In this study,we have synthesized a novel organic compound(PTPZ),comprised of a centrally symmetric and fully ladder-type structure,tailored for aqueous proton storage.This unique configuration imparts the PTPZ molecule with high electron delocalization and enhanced structural stability.As an electrode material,PTPZ demonstrates a substantial proton-storage capacity of 311.9mAh g^(-1),with an active group utilization efficiency of up to 89% facilitated by an 8-electron transfer process,while maintaining a capacity retention of 92.89% after 8000 chargingdischarging cycles.Furthermore,in-situ monitoring technologies and various theoretical analyses have pinpointed the associated electrochemical processes of the PTPZ electrode,revealing exceptional redox activity,rapid proton diffusion,and efficient charge transfer.These attributes confer a significant competitive advantage to PTPZ as an anode material for high-performance proton storage devices.Consequently,this work contributes to the rational design of organic electrode materials for the advancement of rechargeable aqueous batteries.展开更多
Molecular high-order harmonic spectroscopy is a significant advancement in ultrafast science, enabling the measurement of multielectron dynamics with attosecond temporal resolution. The fine structures observed in the...Molecular high-order harmonic spectroscopy is a significant advancement in ultrafast science, enabling the measurement of multielectron dynamics with attosecond temporal resolution. The fine structures observed in the molecular harmonic spectrum provide crucial insights into the structural or multielectron dynamical effects induced by intense laser fields. In this study, we measure the high-order harmonic spectrum of aligned CO_(2) molecules contributed from short trajectories. Two distinct groups of minima are identified in the plateau region. Our findings indicate that the deeper-lying molecular orbitals and two-center interference play significant roles in molecular harmonic generation. The results pave the way for advancing the understanding of multielectron dynamics in polyatomic molecules under intense laser fields.展开更多
As a recently emerging wastewater treatment technology,Algal-bacterial granular sludge(ABGS)process shows significant advantages.However,current research on the ABGS system is a lack of a clear and complete understand...As a recently emerging wastewater treatment technology,Algal-bacterial granular sludge(ABGS)process shows significant advantages.However,current research on the ABGS system is a lack of a clear and complete understanding of the potential mechanism of signal molecules on the growth of ABGS.This study comprehensively explores the variations in the ABGS under different N-acyl-homoserine lactone(AHL)conditions by constructing three sequencing batch reactor(SBR)systems.The results indicate that N-hexanoyl-l-homoserine lactone(C6-HSL)accelerates the granulation process in the early stages by promoting the loosely bound extracellular polymeric substances(LB-EPS)secretion and filamentous bacteria growth,thereby shortening required time for initial granule formation.On the other hand,N-(3-oxodecanoyl)-l-homoserine lactone(3-oxo-C12-HSL)expedites the granulation process by promoting the tightly bound extracellular polymeric substances(TB-EPS)and aromatic protein secretion,benefiting structural stability and nitrogen and phosphorus removal efficiency of mature ABGS.展开更多
Soliton molecules(SMs),bounded and self-assembled of particle-like dissipative solitons,exist with versatile mutual interactions and manifest substantial potential in soliton communication and optical data storage.How...Soliton molecules(SMs),bounded and self-assembled of particle-like dissipative solitons,exist with versatile mutual interactions and manifest substantial potential in soliton communication and optical data storage.However,controllable manipulation of the bounded molecular patterns remains challenging,as reaching a specific operation regime in lasers generally involves adjusting multiple control parameters in connection with a wide range of accessible pulse dynamics.An evolutionary algorithm is implemented for intelligent control of SMs in a 2μm ultrafast fiber laser mode locked through nonlinear polarization rotation.Depending on the specifications of the merit function used for the optimization procedure,various SM operations are obtained,including spectra shape programming and controllable deterministic switching of doublet and triplet SMs operating in stationary or pulsation states with reconfigurable temporal separations,frequency locking of pulsation SMs,doublet and SM complexes with controllable pulsation ratio,etc.Digital encoding is further demonstrated in this platform by employing the self-assembled characteristics of SMs.Our work opens up an avenue for active SM control beyond conventional telecom bands and brings useful insights into nonlinear science and applications.展开更多
基金supported by the National Key Research and Development Program of China(Grant No.2022YFE0134200)the National Natural Science Foundation of China(Grant No.12204214)+1 种基金the Fundamental Research Funds for the Central Universities(Grant No.GK202207012)QCYRCXM-2022-241。
文摘Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and exchangecorrelation effects but also the interference between the dynamics of different electron wave packets.
基金financial support of National Key Research and Development Program of China(Grant No.2022YFB04200302)joint funds of National Natural Science Foundation of China(Grant No.62104115)+5 种基金National Natural Science Foundation of China(Grant No.U21A2072)Overseas Expertise Introduction Project for Discipline Innovation of Higher Education of China(Grant No.B16027)Key R&D Program of Hebei Province(No.19214301D)Yunnan Provincial Science and Technology Project at Southwest United Graduate School(No.202302A0370009)Haihe Laboratory of Sustainable Chemical TransformationsFundamental Research Funds for the Central Universities,Nankai University。
文摘The tensile strain in inorganic perovskite films induced by thermal annealing is one of the primary factors contributing to the inefficiency and instability of inorganic perovskite solar cells(IPSCs),which reduces the defect formation energy.Here,a flexible molecule 5-maleimidovaleric acid(5-MVA)was introduced as a strain buffer to release the residual strain of CsPbI_(2.85)Br_(0.15)perovskite.Maleic anhydride and carboxyl groups in 5-MVA interact strongly with the uncoordinated Pb^(2+)through Lewis acid-base reaction,thus tightly“pull”the perovskite lattice.The in-between soft carbon chain increased the structural flexibility of CsPbI_(2.85)Br_(0.15)perovskite materials,which effectively relieved the intrinsic internal strain of CsPbI_(2.85)Br_(0.15),resisted the corrosion of external strain,and also reduced the formation of defects such as VIand Pb0.In addition,the introduction of 5-MVA improved crystal quality,passivated residual defects,and narrowed energy level barriers.Eventually,power conversion efficiency(PCE)of NiOxbased inverted IPSCs increased from 19.25%to 20.82%with the open-circuit voltage enhanced from 1.164 V to 1.230 V.The release of strain also improved the stability of CsPbI_(2.85)Br_(0.15)perovskite films and devices.
基金supported by the Young Elite Scientists Sponsorship Program by CAST(No.2023QNRC001)Natural Science Foundation of Hunan Province,China(No.2024JJ2074)supported in part by the High Performance Computing Center of Central South University,China and the Pawsey Supercomputing Centre with funding from the Australian Government and the Government of Western Australia.
文摘An in-depth understanding of the hydration mechanism of tricalcium silicate is an important basis for optimizing cement strength development.In this study,the adsorption of water molecules onto the M3-C3S(001)surface at different water coverage levels(θ=1/5,2/5,3/5,4/5,and 1)was investigated using first-principles calculations.The results demonstrate that the conclusions obtained for single water molecule adsorption cannot be fully applied to multiple water molecule adsorption.The total adsorption energies become more negative with increasing water coverage,while the average adsorption energy of each water molecule becomes more positive with increasing water coverage.The water–water interactions reduce the water–surface interactions and are responsible for the anticooperative adsorption of multiple water molecules onto M3-C_(3)S(001).The formation of Ca–OH(–Ca)bonds favors the detachment of Ca from co-valent oxygen,which reveals the significant role of dissociative adsorption.This work aims to extend the water adsorption study on M3-C3S(001)from single water molecule adsorption to multiple water molecule adsorption,providing more detailed insights into the initial water reaction on the C3S surface.
文摘The ring has been a romantic fascination throughout the ages,embodying not only beauty and order but also harboring numerous undisclosed properties awaiting discovery.In the realm of supramolecular chemistry,macrocycles,with a cyclic structure and a central cavity like a doughnut,captivate the attention of scientists[1].In 1967,Pedersen's groundbreaking revelation that alkali metal ions could"fall into"the cavities of a cyclic ether named crown ether,even in organic solvents,unveiled a novel universe of macrocycle chemistry.Since then,numerous macrocyclic structures in nature have been discovered,isolated,and scrutinized.Drawing inspiration from nature,chemists endeavor to explore the vast potential of macrocyclic compounds by designing and synthesizing artificial macrocycles with diverse structural features and recognition properties.
基金support from the National Natural Science Foundation of China(62204146,52303259)the Start-up Grant of Henan University of Technology(2023BS035)。
文摘In recent years,the ternary strategy of adding a vip molecule to the active layer has been proven to be effective for improving the performance of organic solar cells(OSCs).Isomerization engineering of the vip molecule is a simple method to increase the amount of promising material,but there are only limited reports,and the structure-property relationships are still unclear.In this work,we synthesized three isomers named BTA5-F-o,BTA5-F-m,and BTA5-F-p,with different fluorine substitution positions,to study the influence of isomerization on the photovoltaic performance.After introducing them as the third components to the classic host system PM6:Y6,all three ternary devices showed improved power conversion efficiency(PCEs)compared to the binary system(PCE of 17.46%).The ternary OSCs based on BTA5-F-o achieved a champion PCE of 19.11%,while BTA5-F-m and BTA5-F-p realized PCEs of 18.65%and 18.45%,respectively.Mechanism studies have shown that the dipole moment of the BTA5-F-o end group is closer to that of the Y6 end group,despite the three isomers with almost identical energy levels and optical properties.It is indicated that the electron attraction ability of BTA5-F-o best matches that of Y6,which leads to the higher charge mobility,less charge recombination,and stronger exciton dissociation and extraction ability in the ternary blend system.This study suggests that rationally adjusting the position of substituents in the terminal group can be an effective way to construct nonfullerene vip acceptors to achieve highly efficient ternary OSCs.
基金supported by the National Key Research and Development Program of China (Grant No. 2023YFC3706203)the National Natural Science Foundation of China (Grant Nos. 91644214, 22361162668, and 22406109)+1 种基金the China Postdoctoral Science Foundation (Grant No. 2024M751797)Shandong Postdoctoral Science Foundation (SDCX-ZG-202400178)
文摘Enhanced mass concentrations of aromatic-derived secondary organic aerosol(SOA)are frequently observed during humid-haze events.However,the influencing mechanism of relative humidity(RH)in aromatic-derived SOA formation remains incompletely understood.Here,the RH dependence of SOA formation in the presence of NOx was explored by a series of chamber experiments for toluene(TOL)and 1,3,5-trimethylbenzene(TMB)photooxidation.The yield of TOL SOA and TMB SOA increased by 221%and 52%with increasing RH from~8%to~70%,respectively.Analytical results from a high-resolution mass spectrometer showed that SOA constituents with high oxygen content(O/C>0.6)were more abundant in SOA formed in the~70%RH experiment.The elevated yields and O/C of SOA could be attributed to the promoted formation and particle-phase diffusivity of highly oxidized molecules.In addition,in comparison with TMB,TOL could produce more unsaturated aldehydes,which are oxidized into carboxylic acids with high O/C,leading to a more sensitive response of TOL SOA formation to the change in RH.Our work provides mechanistic insights into RH roles in aromatic SOA formation and is helpful for a better understanding of humid-haze events.
文摘This paper provides a systematic review of Matrix-Assisted Laser Desorption/Ionization-Mass Spectrometry Imaging(MALDI-MSI),encompassing its technical principles,experimental workflows,matrix optimization strategies,and recent advancements in plant science applications.It highlights the method's groundbreaking applications in spatial mapping of plant metabolites,dynamic hormone monitoring,and functional studies of tissue microdomains,while offering critical insights into current technical limitations and future research directions.
文摘Acceptor-donor-acceptor(A-D-A)type molecules,of which the novel non-fused azacyclic end-group pyrazoli-nones were modified with chlorine substitution on the phenyl ring,were synthesized.The non-fused azacyclic end-group py-razolinones have the advantages of simple synthesis steps,low cost and environmental friendliness,compared to the classical end-group dicyanomethyleneindianone.The properties of the synthesized A-D-A type molecules with non-fused azacyclic end groups were characterized by theoretical calculation,UV-vis absorption,cyclic voltammetry,X-ray diffraction and space charge limited current.It is shown that the strong UV-vis absorptions of the synthesized A-D-A type molecules are located in the wavelength range of 500~700 nm,with a moderate band gap of nearly 1.7 eV.At the same time,the influence of end-group chlorination on the properties of A-D-A type molecules was compared and explored.It is proven that this kind of A-D-A type molecule with non-fused azacyclic end groups has the potential to be applied as interfacial modified layer of the active layer in perovskite solar cell devices.
基金supported by the National Natural Science Foundation of China(No.22073090,No.21991132,No.52021002)the National Key R&D Program of China(No.2020YFA0710700)the Funds of Youth Innovation Promotion Association,and the Fundamental Research Funds for the Central Universities(WK3450000009).
文摘CRISPR-based tran-scription regulators(CRISPR-TRs)have revolutionized the field of synthetic biol-ogy by enabling tar-geted activation or repression of any de-sired gene.However,the majority of exist-ing inducible CRISPR-TRs are limited by their dependence on specific sequences,which restricts their flex-ibility and controllability in genetic engineering applications.In this study,we proposed a novel strategy to construct sequence-independent inducible CRISPR-TRs,which is achieved by the design of stem loop 2 in the single guide RNA(sgRNA).Under this strategy,by utiliz-ing toehold-mediated strand displacement(TMSD)reactions between small endogenous molecules(miR-20a and TK1 mRNA)and bridge RNA(bRNA)to link bRNA with sgRNA,we achieved synergistic transcriptional activation of VP64 and p65-HSF1 in response to en-dogenous molecules.To enable response to exogenous molecules,we added response se-quences and bRNA sequences to the 5'end of sgRNA to block sgRNA activity,and achieved activation of sgRNA by shearing the response sequence,called sequential unlimited interlock-ing(SUI).Compared with conventional sequence-restricted interlocking(spacer-blocking hairpin(SBH)),the transcriptional activation ratio between response and non-response to the Cas6A protein using our approach was increased by 2.28-fold.Our work presents a modular and versatile framework for endogenous and exogenous molecule-responsive CRISPR-TRs in mammalian cells,without limitations imposed by sequence dependence.
基金supported by the financial support from the National Research Foundation,Singapore,under its Singapore-China Joint Flagship Project(Clean Energy).
文摘Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from the cathode side.These challenges lead to poor cycle stability and severe self-discharge.From the fabrication and cost point of view,it is technologically more viable to deploy electrolyte engineering than electrode protection strategies.More importantly,a synchronous method for modulation of both cathode and anode is pivotal,which has been often neglected in prior studies.In this work,cationic poly(allylamine hydrochloride)(Pah^(+))is adopted as a low-cost dual-function electrolyte additive for ZIBs.We elaborate the synchronous effect by Pah^(+)in stabilizing Zn anode and immobilizing polyiodide anions.The fabricated Zn-iodine coin cell with Pah^(+)(ZnI_(2) loading:25 mg cm^(−2))stably cycles 1000 times at 1 C,and a single-layered 3.4 cm^(2) pouch cell(N/P ratio~1.5)with the same mass loading cycles over 300 times with insignificant capacity decay.
基金the financial support from the Natural Science Foundation of Xiamen,China(3502Z202373075)the National Natural Science Foundation of China(Grant nos.22175180,52311530673,22103013)+1 种基金the Natural Science Foundation of Fujian Province(No.2023J01527,2021J01184,2024J01189)the Start-up funding from Fujian Normal University(Y0720312K13)。
文摘Exploring multifunctional interfacial modifiers is an effective approach to addressing interface issues in perovskite solar cells(PSCs)and improving device performance and stability.While most interfacial modifiers focus on passivating defects at the interfaces,there has been limited investigation into the relationship between molecular design and interfacial charge dynamics.This work introduces resonance molecules with a push-pull effect for interfacial modification,allowing for synergistic regulation of passivation effects and charge dynamics.Specifically,FCz-PO,which includes an electron-withdrawing fluorine atom,exhibits superior passivation but poor molecular stacking and charge extraction.In contrast,MCz-PO,featuring an electron-donating methoxy group,provides effective passivation,wellordered molecular packing,and efficient charge extraction and transport.Consequently,PSCs using MCz-PO achieve high power conversion efficiency(PCE)of 24.74%and excellent operational stability.This study suggests that resonance structures can be an effective molecular design strategy for developing interfacial modifiers with both strong passivation capabilities and well-regulated charge dynamics.
基金supported by the National Natural Science Foun-dation of China(Grant Nos.12475032 and 12005062)the Supercomputing Center of the Chinese Academy of Sciences,Shanghai Snowlake Technology Co.,Ltd.,and the Shanghai Super-Computer Center of China。
文摘Spiral patterns widely exist in both macroscopic and microscopic systems such as hearts,bacteria,and active matters but have never been reported at molecular length scale.The emergence of spiral patterns has considerable impacts on the trajectories of the objects and thus usually relates to various physical,chemical,biological and physiological processes.In this paper,we show that,down to the length scale of only several Angstroms,asymmetric molecules exhibit spiral patterns in their trajectories within finite time based on the under-damped Langevin equation and demonstrated by molecular dynamics simulation.The key to this observation lies in the asymmetric molecular architecture that leads to a translation-rotation coupling.This finding enriches the knowledge of spiral patterns to the molecular length scale,provides a new insight into the understanding of various processes at the molecular level,and may evoke new ideas on the understanding of the vortices in turbulence.
基金the Yunnan Fundamental Research Projects(Grant Nos.202501AT070298,202401AU070163,and 202401AT070368)the National Natural Science Foundation of China(Grant No.52162030)+5 种基金the Yunnan Major Scientific and Technological Projects(Grant No.202202AG050003)the Yunnan Engineering Research Center Innovation Ability Construction and Enhancement Projects(Grant No.2023-XMDJ-00617107)the University Service Key Industry Project of Yunnan Province(Grant No.FWCY-ZD2024005)the Yunnan Thousand Talents Program for Young Talents(Grant No.KKS2202052001)the Scientific Research Foundation of Kunming University of Science and Technology(Grant No.20220122)the Analysis and Testing Foundation of Kunming University of Science and Technology(Grant No.2023T20220122).
文摘The presence of residual alkaline compounds in the ultrahigh-nickel layered oxide cathodes(LiNi_(x)Co_(y)Mn_(1−x−y)O_(2),x≥_(0.9))aggravates structural degradation,increases surface reactivity,and promotes slurry gelation,leading to the capacity decay of batteries with these cathodes and complicating their manufacturing.Traditional approaches for addressing this issue,including direct removal,coverage,and utilization,are complex and require surface regeneration.Herein,we propose neutralizing residual alkaline compounds with 3-thiopheneboronic acid(3-TBA)to improve the performance of LiNi_(0.9)5Co_(0.04)Mn_(0.01)O_(2)(NCM)cathode material,a facile strategy that does not require any post-treatment.The suggested reaction yields a uniform and thin organic-modified layer on the surface of the NCM cathode,improving its chemical stability toward the electrolyte,as demonstrated by multiple characterization methods.The modified NCM cathode exhibited impressive cyclic and rate performances,achieving a capacity retention of 83.34%after 200 cycles at 1.0 C and a specific capacity of 162.00 mAh·g^(−1) at 10.0 C.Most importantly,the proposed approach can efficiently suppress unfavorable phase transitions,severe electrolyte degradation,and CO_(2) gas evolution,improving the application potential of ultrahigh-nickel layered oxide cathode materials.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12174115 and 91836103)。
文摘We propose a scheme for dual-species deceleration and trapping of a cold atom–molecule mixture by a frequency chirping stimulated force.We study the stimulated force exerted on Mg F and Rb using optical Bloch equations based on a direct numerical solution for the time-dependent density matrix.We analyze the relationship between the frequency chirping rate and the number of Mg F molecules and Rb atoms.In addition,we study the dynamical process of molecular deceleration and the effect of transverse diffusion.Monte–Carlo simulations show that buffer-gas-cooled Mg F and Rb beams,with initial velocities of 200 m/s and 130 m/s respectively,can be decelerated to less than 10 m/s.This is achieved with laser powers of as low as 357 m W for Mg F and 10 m W for Rb per traveling wave.The rapid deceleration minimizes molecular loss due to transverse diffusion during the deceleration process.The estimated number of molecules that can be trapped in a magneto-optical trap(MOT)is about 9.0×10^(6),which is an order of magnitude larger than the number of Mg F molecules decelerated by the spontaneous radiation force.The results offer a promising starting point for further studies of sympathetic cooling.
基金Project supported by the National Natural Science Foundation of China(Grant No.62175116)。
文摘Recent theoretical verification of self-similar and dissipative pure-quartic solitons(PQSs)emphasized the similarity between PQS lasers and conventional fiber lasers,but the unique equilibrium mechanism hinders the formation of PQS molecules in normal fourth-order dispersion(FOD)regimes.In this paper,we investigated the effect of filters on shaping PQSs in normal FOD based on a passively mode-locked fiber laser model.A bandpass filter eliminates the time pedestal of dissipative PQSs,thus realizing a multi-pulsing state.When the filter bandwidth is appropriate,the effective spectral filtering effect can lower the pulse splitting threshold and enable the coherent restoration from chaotic PQSs to PQS molecules.Additionally,changing the central wavelength of the filter can generate PQSs and PQS molecules with asymmetric intensity distributions.These results are important guides for the manipulation of PQSs and the construction of high repetition-frequency fiber lasers.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 12174115 and 91836103)。
文摘We present a theoretical approach to achieve sub-Doppler cooling of magnesium fluoride(Mg F) molecules by tuning the AC Stark shift with a blue-detuned laser. We study three blue-detuned magneto–optical trapping(MOT) schemes by using the Bayesian optimization method with the optical Bloch equations. We perform a comprehensive analysis of the relationship between the force in the MOT and the velocities and positions of the Mg F molecules. Monte–Carlo simulations show that our MOT schemes can achieve a temperature as low as 28 μK and a density as high as 4.0 × 10^(8)cm^(-3) at the conditions of a ratio of two laser intensities of 2:7, a detuning of 3Γ and a polarization configuration of σ^(-)-σ^(+). These results provide a clear way for transferring a large number of Mg F molecules into a conservative trap to enhance the subsequent cooling such as evaporative or sympathetic cooling.
基金National Natural Science Foundation of China,Grant/Award Numbers:22279166,52002157National Institute of Education,Singapore,under its Academic Research Fund,Grant/Award Numbers:RI 1/21 EAH,RI 3/23 EAH+1 种基金China Postdoctoral Science Foundation,Grant/Award Numbers:2022M711686,2023M741471Postgraduate Research&Practice Innovation Program of Jiangsu Province,Grant/Award Number:SJCX24_2512。
文摘The architectural design of redox-active organic molecules and the modulation of their electronic properties significantly influence their application in energy storage systems within aqueous environments.However,these organic molecules often exhibit sluggish reaction kinetics and unsatisfactory utilization of active sites,presenting significant challenges for their practical deployment as electrode materials in aqueous batteries.In this study,we have synthesized a novel organic compound(PTPZ),comprised of a centrally symmetric and fully ladder-type structure,tailored for aqueous proton storage.This unique configuration imparts the PTPZ molecule with high electron delocalization and enhanced structural stability.As an electrode material,PTPZ demonstrates a substantial proton-storage capacity of 311.9mAh g^(-1),with an active group utilization efficiency of up to 89% facilitated by an 8-electron transfer process,while maintaining a capacity retention of 92.89% after 8000 chargingdischarging cycles.Furthermore,in-situ monitoring technologies and various theoretical analyses have pinpointed the associated electrochemical processes of the PTPZ electrode,revealing exceptional redox activity,rapid proton diffusion,and efficient charge transfer.These attributes confer a significant competitive advantage to PTPZ as an anode material for high-performance proton storage devices.Consequently,this work contributes to the rational design of organic electrode materials for the advancement of rechargeable aqueous batteries.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 92250306 and 12304302)the Natural Science Foundation of Jilin Province, China (Grant Nos. YDZJ202101ZYTS157 and YDZJ202201ZYTS314)the Scientific Research Foundation of Jilin Province Education Department, China (Grant No. JJKH20230283KJ)。
文摘Molecular high-order harmonic spectroscopy is a significant advancement in ultrafast science, enabling the measurement of multielectron dynamics with attosecond temporal resolution. The fine structures observed in the molecular harmonic spectrum provide crucial insights into the structural or multielectron dynamical effects induced by intense laser fields. In this study, we measure the high-order harmonic spectrum of aligned CO_(2) molecules contributed from short trajectories. Two distinct groups of minima are identified in the plateau region. Our findings indicate that the deeper-lying molecular orbitals and two-center interference play significant roles in molecular harmonic generation. The results pave the way for advancing the understanding of multielectron dynamics in polyatomic molecules under intense laser fields.
基金financially supported by the Open Project of Sanya Science and Education Innovation Park of Wuhan University of Technology(No.2022KF0005)Researchers Supporting Project(No.RSP-2024-R20)King Saud University,Riyadh,Saudi Arabia.
文摘As a recently emerging wastewater treatment technology,Algal-bacterial granular sludge(ABGS)process shows significant advantages.However,current research on the ABGS system is a lack of a clear and complete understanding of the potential mechanism of signal molecules on the growth of ABGS.This study comprehensively explores the variations in the ABGS under different N-acyl-homoserine lactone(AHL)conditions by constructing three sequencing batch reactor(SBR)systems.The results indicate that N-hexanoyl-l-homoserine lactone(C6-HSL)accelerates the granulation process in the early stages by promoting the loosely bound extracellular polymeric substances(LB-EPS)secretion and filamentous bacteria growth,thereby shortening required time for initial granule formation.On the other hand,N-(3-oxodecanoyl)-l-homoserine lactone(3-oxo-C12-HSL)expedites the granulation process by promoting the tightly bound extracellular polymeric substances(TB-EPS)and aromatic protein secretion,benefiting structural stability and nitrogen and phosphorus removal efficiency of mature ABGS.
基金supported by the Research Grants Council of the Hong Kong Special Administrative Region of China(Grant Nos.HKU 17212824,HKU 17210522,HKU C7074-21G,HKU R7003-21,and HKU 17205321)the Innovation and Technology Commission of the Hong Kong SAR Government(Grant Nos.MHP/073/20 and MHP/057/21),and the Health@InnoHK program.
文摘Soliton molecules(SMs),bounded and self-assembled of particle-like dissipative solitons,exist with versatile mutual interactions and manifest substantial potential in soliton communication and optical data storage.However,controllable manipulation of the bounded molecular patterns remains challenging,as reaching a specific operation regime in lasers generally involves adjusting multiple control parameters in connection with a wide range of accessible pulse dynamics.An evolutionary algorithm is implemented for intelligent control of SMs in a 2μm ultrafast fiber laser mode locked through nonlinear polarization rotation.Depending on the specifications of the merit function used for the optimization procedure,various SM operations are obtained,including spectra shape programming and controllable deterministic switching of doublet and triplet SMs operating in stationary or pulsation states with reconfigurable temporal separations,frequency locking of pulsation SMs,doublet and SM complexes with controllable pulsation ratio,etc.Digital encoding is further demonstrated in this platform by employing the self-assembled characteristics of SMs.Our work opens up an avenue for active SM control beyond conventional telecom bands and brings useful insights into nonlinear science and applications.
